In 1967, he starred in action movieThe Venetian Affair, directed by Jerry Thorpe. A year later, he had a role in Bullitt (1968), with Steve McQueen. For this work Robert Vaughn was nominated for a BAFTA Award, for "Best Supporting Actor". In 1969 he starred with George Segal, in the war movie The Bridge at Remagen (1969). Then in 1970, has the role of Servilius Casca in Julius Caesar, with Charlton Heston.

Success was so great that there were several movies. These included To Trap a Spy (1964), The Spy with My Face (1965), One Spy Too Many (1966), One of Our Spies is Missing (1966), The Spy in the Green Hat (1966), The Karate Killers (1967), The Helicopter Spies (1968), How to Steal the World (1968).

In 1983 Vaughn and McCallum were reunited for the TV movie The Return of the Man from U.N.C.L.E.: The Fifteen Years Later Affair.

In 1965 and 1966 Robert Vaughn was nominated twice for the Golden Globe Award as Best TV Star - Male for The Man from U.N.C.L.E.

In 1963 he starred in her first television series The Lieutenant, as Captain Ray Rambridge. In 1970s worked in the TV mini-seriesCaptains and the Kings (1976), Washington: Behind Closed Doors (1977), and Centennial (1978-1979). Robert Vaughn also worked for the British television. He starred in series The Protectors (1972-1974). Vaughn played the role of Harry Rule for 52 episodes of the series. In 1986, he was hired to play the role of General Hunt Stockwell, in The A-Team, with George Peppard.

He also worked in the television westernThe Magnificent Seven (1998) as Judge Oren Travis.